Complementary use of monochromatic and white-beam X-ray micro-diffraction for the investigation of ancient materials
Abstract
Archaeological artefacts are often heterogeneous materials where several phases coexist in a wide grain size distribution. Most of the time, retrieving structure information at the micrometre scale is of great importance for these materials. Particularly, the organization of different phases at the micrometre scale is closely related to optical or mechanical properties, manufacturing processes, functionalities in ancient times and long-term conservation. Between classic X-ray powder diffraction with a millimetre beam and transmission electron microscopy, a gap exists and structure and phase information at the micrometre scale are missing. Using a micrometre-size synchrotron X-ray beam, a hybrid approach combining both monochromatic powder micro-diffraction and Laue single-crystal micro-diffraction was deployed to obtain information from nanometre- and micrometre-size phases, respectively. Therefore providing a way to bridge the aforementioned gap, this unique methodology was applied to three different types of ancient materials that all show a strong heterogeneity. In Roman terra sigillata, the specific distribution of nanocrystalline hematite is mainly responsible for the deep-red tone of the slip, while the distribution of micrometre-size quartz in ceramic bodies reflects the change of manufacturing process between pre-sigillata and high-quality sigillata periods. In the second example, we investigated the modifications occurring in Neolithic and geological flints aftermore »
- Authors:
-
- ETH Zurich, Zurich (Switzerland)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- CNRS - Univ. de Poitiers - ENSMA, Futuroscope (France)
- CEMES - CNRS - Univ. de Toulouse, Toulouse (France)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1392969
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Applied Crystallography (Online)
- Additional Journal Information:
- Journal Name: Journal of Applied Crystallography (Online); Journal Volume: 48; Journal Issue: 5; Journal ID: ISSN 1600-5767
- Publisher:
- International Union of Crystallography
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; cultural heritage materials; Laue microdiffraction; powder microdiffraction; grain size; residual strain
Citation Formats
Dejoie, Catherine, Tamura, Nobumichi, Kunz, Martin, Goudeau, Philippe, and Sciau, Philippe. Complementary use of monochromatic and white-beam X-ray micro-diffraction for the investigation of ancient materials. United States: N. p., 2015.
Web. doi:10.1107/S1600576715014983.
Dejoie, Catherine, Tamura, Nobumichi, Kunz, Martin, Goudeau, Philippe, & Sciau, Philippe. Complementary use of monochromatic and white-beam X-ray micro-diffraction for the investigation of ancient materials. United States. https://doi.org/10.1107/S1600576715014983
Dejoie, Catherine, Tamura, Nobumichi, Kunz, Martin, Goudeau, Philippe, and Sciau, Philippe. Sun .
"Complementary use of monochromatic and white-beam X-ray micro-diffraction for the investigation of ancient materials". United States. https://doi.org/10.1107/S1600576715014983. https://www.osti.gov/servlets/purl/1392969.
@article{osti_1392969,
title = {Complementary use of monochromatic and white-beam X-ray micro-diffraction for the investigation of ancient materials},
author = {Dejoie, Catherine and Tamura, Nobumichi and Kunz, Martin and Goudeau, Philippe and Sciau, Philippe},
abstractNote = {Archaeological artefacts are often heterogeneous materials where several phases coexist in a wide grain size distribution. Most of the time, retrieving structure information at the micrometre scale is of great importance for these materials. Particularly, the organization of different phases at the micrometre scale is closely related to optical or mechanical properties, manufacturing processes, functionalities in ancient times and long-term conservation. Between classic X-ray powder diffraction with a millimetre beam and transmission electron microscopy, a gap exists and structure and phase information at the micrometre scale are missing. Using a micrometre-size synchrotron X-ray beam, a hybrid approach combining both monochromatic powder micro-diffraction and Laue single-crystal micro-diffraction was deployed to obtain information from nanometre- and micrometre-size phases, respectively. Therefore providing a way to bridge the aforementioned gap, this unique methodology was applied to three different types of ancient materials that all show a strong heterogeneity. In Roman terra sigillata, the specific distribution of nanocrystalline hematite is mainly responsible for the deep-red tone of the slip, while the distribution of micrometre-size quartz in ceramic bodies reflects the change of manufacturing process between pre-sigillata and high-quality sigillata periods. In the second example, we investigated the modifications occurring in Neolithic and geological flints after a heating process. By separating the diffracted signal coming from the nano- and the micrometre scale, we observed a domain size increase for nanocrystalline quartz in geological flints and a relaxation of the residual strain in larger detritic quartz. In conclusion, through the study of a Roman iron nail, we showed that the carburation process to strengthen the steel was mainly a surface process that formed 10–20 µm size domains of single–crystal ferrite and nanocrystalline cementite.},
doi = {10.1107/S1600576715014983},
journal = {Journal of Applied Crystallography (Online)},
number = 5,
volume = 48,
place = {United States},
year = {Sun Sep 20 00:00:00 EDT 2015},
month = {Sun Sep 20 00:00:00 EDT 2015}
}
Web of Science
Works referenced in this record:
The Influence of Aluminum on Iron Oxides. Part II. Preparation and Properties of Al-Substituted Hematites
journal, January 1979
- Schwertmann, U.
- Clays and Clay Minerals, Vol. 27, Issue 2
A superbend X-ray microdiffraction beamline at the advanced light source
journal, October 2009
- Tamura, N.; Kunz, M.; Chen, K.
- Materials Science and Engineering: A, Vol. 524, Issue 1-2
Mesoscale x-ray diffraction measurement of stress relaxation associated with buckling in compressed thin films
journal, July 2003
- Goudeau, Philippe; Villain, Pascale; Tamura, Nobumichi
- Applied Physics Letters, Vol. 83, Issue 1
Micro-Raman study of aluminium-bearing hematite from the slip of Gaulsigillata wares
journal, January 2006
- Zoppi, A.; Lofrumento, C.; Castellucci, E. M.
- Journal of Raman Spectroscopy, Vol. 37, Issue 10
Evolution of terra sigillata technology from Italy to Gaul through a multi-technique approach
journal, January 2015
- Leon, Yoanna; Sciau, Philippe; Passelac, Michel
- Journal of Analytical Atomic Spectrometry, Vol. 30, Issue 3
Influence of Taoism on the invention of the purple pigment used on the Qin terracotta warriors
journal, November 2007
- Liu, Z.; Mehta, A.; Tamura, N.
- Journal of Archaeological Science, Vol. 34, Issue 11
Sub-micrometre depth-gradient measurements of phase, strain and texture in polycrystalline thin films: a nano-pencil beam diffraction approach
journal, February 2014
- Vaxelaire, Nicolas; Gergaud, Patrice; Vaughan, Gavin B. M.
- Journal of Applied Crystallography, Vol. 47, Issue 2
Making make-up in Ancient Egypt
journal, February 1999
- Walter, P.; Martinetto, P.; Tsoucaris, G.
- Nature, Vol. 397, Issue 6719
Crystal Structure of an Indigo@Silicalite Hybrid Related to the Ancient Maya Blue Pigment
journal, November 2014
- Dejoie, Catherine; Martinetto, Pauline; Tamura, Nobumichi
- The Journal of Physical Chemistry C, Vol. 118, Issue 48
A study of the Roman iron bars of Saintes-Maries-de-la-Mer (Bouches-du-Rhône, France). A proposal for a comprehensive metallographic approach
journal, June 2011
- Pagès, G.; Dillmann, P.; Fluzin, P.
- Journal of Archaeological Science, Vol. 38, Issue 6
Raman spectroscopy in art and archaeology
journal, August 2008
- Baraldi, Pietro; Tinti, Anna
- Journal of Raman Spectroscopy, Vol. 39, Issue 8
Petrography of geomaterials: a review
journal, November 2011
- Ingham, J. P.
- Quarterly Journal of Engineering Geology and Hydrogeology, Vol. 44, Issue 4
Nature and Microstructure of Gallic Imitations of Sigillata Slips from the la Graufesenque Workshop*
journal, October 2009
- Mirguet, C.; Dejoie, C.; Roucau, C.
- Archaeometry, Vol. 51, Issue 5
Microstructural and Microchemical Characterization of Roman Period Terra Sigillate Slips from Archeological Sites in Southern France
journal, March 2006
- Sciau, Philippe; Relaix, Sabrina; Roucau, Christian
- Journal of the American Ceramic Society, Vol. 89, Issue 3
Micrometer-scale synchrotron diffraction mapping analysis of carbide precipitation in deep cryogenically treated low carbon steel
journal, May 2012
- Xu, Ning; Cavallaro, Giuseppe P.; Gerson, Andrea R.
- Journal of Materials Research, Vol. 27, Issue 16
Submicron x-ray diffraction and its applications to problems in materials and environmental science
journal, March 2002
- Tamura, N.; Celestre, R. S.; MacDowell, A. A.
- Review of Scientific Instruments, Vol. 73, Issue 3
Influence of Aluminum Substitution on the Color of Synthetic Hematites
journal, January 1984
- Barron, V.
- Clays and Clay Minerals, Vol. 32, Issue 2
Recent advances in magnetic structure determination by neutron powder diffraction
journal, October 1993
- Rodríguez-Carvajal, Juan
- Physica B: Condensed Matter, Vol. 192, Issue 1-2
TEM characterization of the fine scale microstructure of a Roman ferrous nail
journal, June 2010
- Douin, J.; Henry, O.; Dabosi, F.
- The European Physical Journal Applied Physics, Vol. 51, Issue 1
Submicron X-ray diffraction
journal, July 2001
- MacDowell, A. A.; Celestre, R. S.; Tamura, N.
- Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 467-468
Learning from the past: Rare ε-Fe2O3 in the ancient black-glazed Jian (Tenmoku) wares
journal, May 2014
- Dejoie, Catherine; Sciau, Philippe; Li, Weidong
- Scientific Reports, Vol. 4, Issue 1
Application of white-beam X-ray microdiffraction for the study of mineralogical phase identification in ancient Egyptian pigments
journal, November 2007
- Lynch, P. A.; Tamura, N.; Lau, D.
- Journal of Applied Crystallography, Vol. 40, Issue 6
The visible diffuse reflectance spectrum in relation to the color and crystal properties of hematite
journal, June 2003
- Torrent, José; Barrón, Vidal
- Clays and Clay Minerals, Vol. 51, Issue 3
XMAS: A Versatile Tool for Analyzing Synchrotron X-ray Microdiffraction Data
book, April 2014
- Tamura, Nobumichi
- Strain and Dislocation Gradients from Diffraction
Spectral and other physicochemical properties of submicron powders of hematite (α-Fe 2 O 3 ), maghemite (γ-Fe 2 O 3 ), magnetite (Fe 3 O 4 ), goethite (α-FeOOH), and lepidocrocite (γ-FeOOH)
journal, January 1985
- Morris, Richard V.; Lauer, Howard V.; Lawson, Charles A.
- Journal of Geophysical Research, Vol. 90, Issue B4
Can Laue microdiffraction be used to solve and refine complex inorganic structures?
journal, November 2013
- Dejoie, Catherine; McCusker, Lynne B.; Baerlocher, Christian
- Journal of Applied Crystallography, Vol. 46, Issue 6
Non-destructive synchrotron X-ray diffraction mapping of a Roman painting
journal, September 2005
- Dooryhée, E.; Anne, M.; Bardiès, I.
- Applied Physics A, Vol. 81, Issue 4
A dedicated superbend x-ray microdiffraction beamline for materials, geo-, and environmental sciences at the advanced light source
journal, March 2009
- Kunz, Martin; Tamura, Nobumichi; Chen, Kai
- Review of Scientific Instruments, Vol. 80, Issue 3
Micro X-ray diffraction and fluorescence tomography for the study of multilayered automotive paints
journal, May 2010
- De Nolf, Wout; Janssens, Koen
- Surface and Interface Analysis, Vol. 42, Issue 5
Micro scanning X-ray diffraction study of Gallo-Roman Terra Sigillata ceramics
journal, February 2006
- Sciau, P.; Goudeau, P.; Tamura, N.
- Applied Physics A, Vol. 83, Issue 2
Probing Deformation Substructure by Synchrotron X-ray Diffraction and Dislocation Dynamics Modelling
journal, September 2010
- Korsunsky, Alexander M.; Hofmann, Felix; Song, Xu
- Journal of Nanoscience and Nanotechnology, Vol. 10, Issue 9
The nature of marbled Terra Sigillata slips: a combined μXRF and μXRD investigation
journal, March 2010
- Leon, Y.; Sciau, P.; Goudeau, P.
- Applied Physics A, Vol. 99, Issue 2
Tutorial on x-ray microLaue diffraction
journal, November 2009
- Ice, Gene E.; Pang, Judy W. L.
- Materials Characterization, Vol. 60, Issue 11
Classification of lead white pigments using synchrotron radiation micro X-ray diffraction
journal, August 2007
- Welcomme, E.; Walter, P.; Bleuet, P.
- Applied Physics A, Vol. 89, Issue 4
Three-dimensional X-ray structural microscopy with submicrometre resolution
journal, February 2002
- Larson, B. C.; Yang, Wenge; Ice, G. E.
- Nature, Vol. 415, p. 887-890
Scanning X-ray microdiffraction with submicrometer white beam for strain/stress and orientation mapping in thin films
journal, February 2003
- Tamura, N.; MacDowell, A. A.; Spolenak, R.
- Journal of Synchrotron Radiation, Vol. 10, Issue 2
Full local elastic strain tensor from Laue microdiffraction: simultaneous Laue pattern and spot energy measurement
journal, July 2011
- Robach, Odile; Micha, Jean-Sébastien; Ulrich, Olivier
- Journal of Applied Crystallography, Vol. 44, Issue 4
Evidence for residual elastic strain in deformed natural quartz
journal, June 2009
- Kunz, M.; Chen, K.; Tamura, N.
- American Mineralogist, Vol. 94, Issue 7
Tools for production, goods for reproduction. The function of knapped stone tools at the Neolithic necropolis of Can Gambus-1 (Sabadell, Spain)
journal, September 2012
- Gibaja, Juan F.; Terradas, Xavier
- Comptes Rendus Palevol, Vol. 11, Issue 6
Nanoquartz vs. macroquartz: a study of the α↔β phase transition
journal, March 2001
- Rıos, S.; Salje, E. K. H.; Redfern, S. A. T.
- The European Physical Journal B, Vol. 20, Issue 1
DETECTING AND QUANTIFYING HEAT TREATMENT OF FLINT AND OTHER SILICA ROCKS: A NEW NON-DESTRUCTIVE METHOD APPLIED TO HEAT-TREATED FLINT FROM THE NEOLITHIC CHASSEY CULTURE, SOUTHERN FRANCE: Heat treatment of flint from the Chassey culture, southern France
journal, August 2012
- Schmidt, P.; LÉA, V.; Sciau, Ph.
- Archaeometry, Vol. 55, Issue 5
Unambiguous indexing of trigonal crystals from white-beam Laue diffraction patterns: application to Dauphiné twinning and lattice stress mapping in deformed quartz
journal, August 2012
- Chen, Kai; Dejoie, Catherine; Wenk, Hans-Rudolf
- Journal of Applied Crystallography, Vol. 45, Issue 5
A comparative study of the thermal behaviour of length-fast chalcedony, length-slow chalcedony (quartzine) and moganite
journal, February 2013
- Schmidt, Patrick; Slodczyk, Aneta; Léa, Vanessa
- Physics and Chemistry of Minerals, Vol. 40, Issue 4
The Race to X-ray Microbeam and Nanobeam Science
journal, December 2011
- Ice, G. E.; Budai, J. D.; Pang, J. W. L.
- Science, Vol. 334, Issue 6060
Raw, pre-heated or ready to use: discovering specialist supply systems for flint industries in mid-Neolithic (Chassey culture) communities in southern France
journal, March 2005
- Léa, Vanessa
- Antiquity, Vol. 79, Issue 303
Works referencing / citing this record:
X‐ray Diffraction Mapping for Cultural Heritage Science: a Review of Experimental Configurations and Applications
journal, November 2019
- Gonzalez, Victor; Cotte, Marine; Vanmeert, Frederik
- Chemistry – A European Journal, Vol. 26, Issue 8
Thermal analysis and multi-analytical comparison of samples of Neolithic ceramics from Dnepr–Dvina and Low Don regions
journal, August 2019
- Zvereva, Irina A.; Kuznetsov, Viktor M.; Zhukov, Yuriy M.
- Journal of Thermal Analysis and Calorimetry, Vol. 138, Issue 3
The mechanical properties of heat-treated rocks: a comparison between chert and silcrete
journal, September 2018
- Schmidt, Patrick; Buck, Gerald; Berthold, Christoph
- Archaeological and Anthropological Sciences, Vol. 11, Issue 6
Lattice strain and tilt mapping in stressed Ge microstructures using X-ray Laue micro-diffraction and rainbow filtering
journal, August 2016
- Tardif, Samuel; Gassenq, Alban; Guilloy, Kevin
- Journal of Applied Crystallography, Vol. 49, Issue 5
The status of imported Barremian-Bedoulian flint in north-eastern Iberia during the Middle Neolithic. Insights from the variscite mines of Gavà (Barcelona)
journal, November 2019
- Borrell, Ferran; Bosch, Josep; Gibaja, Juan Francisco
- PLOS ONE, Vol. 14, Issue 11
Quantitative microstructural imaging by scanning Laue x-ray micro- and nanodiffraction
journal, June 2016
- Chen, Xian; Dejoie, Catherine; Jiang, Tengfei
- MRS Bulletin, Vol. 41, Issue 6